Electrochemical process



Jan. 29, 1952 I L. H. SMITH 2,583,899

ELECTROCHEMICAL PROCESS Filed Nov. 29, 1950 2 SHEETSSHEET 1 FIG. 2

- INVENTOR.

1952 1., H. SMITH ELECTROCHEMICAL PROCESS 2 SHEETSSHEET 2 Filed Nov. 291950 FIG. 4

was

FIG.5

INVENTOR. L Q S 0 Patented Jan. 29, 1952 UNTED STATES PATENT OFFICEELECTROCHEMICAL PROCESS- Lester H. Smith, Maplewood, N. J.

Application November 29, 1950, Serial No. 198,081

(Cl. 204-164) I 9 Claims.

1 This invention is concerned with an improved method of producingelectrochemical reactions in gases or suspensions in gases by means ofpassing electrically charged material particles through the gas orsuspension, and at the same time subjecting the gas or suspension andelectrically charged particles to a high frequency electrostatic orelectromagnetic field.

This application is a continuation in part of my application No. 613,174now abandoned.

Considerable experimental work has been done in the field ofelectro-chemistry of gaseous systems using high frequency electrostaticor elecmechanically projecting material particles into a gas such as thespraying of liquid particles from a nozzle or projecting liquid or solidparticles from vibrating or rotating surfaces into a gas, electricallycharging these particles by electrostatic induction as they areprojected and subjecting the drifting charged particles and surroundinggas to a high frequency electric field.

In this application as well as my divisional applications, I have usedthe expression electric space charges to describe an accumulation ofelectrically charged material particles, either liquid or solid,drifting in space between electrodes in the apparatus. At the same time,I also refer to electric charges which may become attached to gasmolecules if electrically charged material particles are evaporated orgasified in space.

Substances which are in a gaseous state are in their molecular form, andthe method of bringing about evaporation or gasification of electricallycharged liquid particles in space by means about by electron emissionfrom cathode surfaces, but is by dispersion and attachment to gasmolecules of electric charges originating in gasified electricallycharged liquid particles. The influence of a high frequency electricfield on gas ions and transient free electric charges is to producemotion of gas ions and circulating currents in a gas mixture. Obviously,this method is much more effective in producing gas phase chemicalreactions than the use of high frequency electric fields only throughgases at low pressures.

The principal object of this invention is to combine the effect of anelectric space charge, as defined previously, and a high frequencyelectrostatic or electromagnetic field on various gases or suspensionsin gases. The said gases in the zone of reaction may include ionized gasderived from the gasiflcation in space of electrically charged particlessuch as liquid spray particles.

Other objects of this invention will be apparent from the drawings andthe following description of the features of the invention and in theprovision of apparatus and methods of operation for accomplishing theforegoing object.

As specifically stated in the claims, theinterelectrode potentials arelimited to values such that direct interelectrode breakdown typeunidirectional discharging does not take place. In other words, whatevercurrent passes between the electrodes in the apparatus isderived-principally from electric charges on material particlesprojected into the gas in the reaction zone. This will be made clear inconnection with the description of the drawings. Breakdown potentialsbetween electrodes in air and in the common gases are of the order of20,000 volts per centimeter. Such breakdown potentials vary to a minordegree between gases. For a given gas they increase slightly withincreased gas density and decrease substantially for high frequencypotentials. Breakdown potentials or ionization potentials of the commongases including many hydrocarbons are well known to those skilled in theart.

The unidirectional potential differences, electrode spacings and otheroperating conditions illustrated in connection with the several figuresare intended to give potential gradients which are well below breakdownvalues.

In accordance with one modification of my invention, electricallycharged material particles are projected from an emitting electrodewhich may be a nozzle, a vibratory plate, or a rotating surface.Necessary electrostatic fields to induce the flow of electric charges onthe projected particles are set up by an intermediate electrode in closeproximity to the emitting electrode and by a collecting electrodelocated at a proper distance from the emitting electrode. Interelectrodeunidirectional potential differences are maintained at suitable valuesso as to promote a drift of the charged particles toward the collectingelectrode which also may provide an external electrical return circuitto the emitting electrode.

At the same time, a flow of gas or of a gas containing a suspension ismaintained through the apparatus housing these electrodes. This flow ofgas may contribute to the driftof charged pardirect current potentials.a high frequency poten-v tial source is connected between the emittingelectrode or intermediate electrode and the col- 'ticles previouslymentioned. In addition tothe to tneupper surface of plate electrode 5..10

frequency electrostatic ,field which are separate from the electrodesused .to'produce the unidiectio al p t t a g adi nt. are usedaccordancewith a third modification .of my nvent on. a pace charg is Produ ed in tam manner as described in connection, with the first m d cation. by t ep ojec in o ec rica y charged material particles from an'emittingelectrode combination with an intermediate electrode and a collectingelectrode.

This spa cha ge pa sed h o h 0.1." n clo e p o t to a h gh equenc windig wh ch generates a high frequency magnetic field. At the same time a fow of s or of a s contain a u pen o is maintained through the same pathtraveled b the drif i g spa e cha ge.

In each of the above modifications when the ir i lationoi gas hrough thapparatus. is in I the same direction as $1 6 .dlift of chargedmaterialparticles, this flow of gas may contribute to the Said drift.The flow of gas through the apparatus may be counten-current to theproie n 9 harged, par ic es ith p op r pr p tioning of the potentialgradien s nd gas velocities.

Referring to the drawings;

Figure l is an illustration of a preferred form of space charge devicein which the same electrode are used for setting up both the unidirec",tional electrostatic fields and the high frequency e ostat c fie d,

Figure 2 shows a modification of Figure l in which the entering gas maypass through the emitting electrode which is perforated. Furthermore,separate electrodes are provided for setting up the high frequencyelectrostatic field.

In Figure 3 is shown a preferred form of space charge device in whichthe drifting space charge and the gas or suspension circulating throughthe device are subjected to a high frequency electr magn t c fi V Figure{1 shows a typical intermediate electrode used in the device of 3.

In Figure 5 is illustrated an alternative arrangement of the highfrequency electromagnetic winding of Fig. 3.

Figure 6 shows a form of rotating emitting electrode which can beutilized in either Fig. 1 or Fig. 3 in place Of the vibratory emittingelectrodes shown.

In Fig. 1 the vessel l is constructed of electrically non-conductingmaterial such as glass sections or solvent resistant plastic material.Vase sel l is provided with agas inlet 2 and processed gas outlet 3 anddrain outlet 4. A flexible cir-v cular metal plate electrode 5 in theupper portion of vessel I is supported from insulating collar 23 d iscon c ed o he ower end of t e s af 6 which turn connected to a source "Iof intermittent vertical vibratory motion of approximately cycles persecond, operating on a cycle of on for 2 seconds and off for 2 seconds.lihe plate electrode 5 is the emitting electrode and is supplied with afluid used to form charged particles through the tube 3. The tube 8passes downward through the top of vessel 3 and makes a right angle bendand runs horizontally close The tube 8 has a slot 9 in the lowersurface. A slot 10 is also provided in the plate electrode 5 close tothe slot 9 in tube 8. In between the periods of vibration of emittingelectrode 5, additional I fluid is supplied through tube 8 and slots 9and ii! and runs downhill on the lower surface of plate electrode 5covering this surface with a thin film of liquid. This film of liquid isprojected downward as tiny droplets on vibration of the plate electrode5. If required, electrode 5 may be provided with perforations at the.lowest point to prevent liquid accumulation above the electrode.

Ages-tight sleeve 11 in the top of vessel i permits vertical motion ofthe shaft 6.. An intermediate electrode 12 of inch spacing inch diameterwire mesh is located close to the lower surface of emitting electrode 5,also a collecting electrode 13 in theform of a screen. Electrode I3 issupported by an insulator I l and insulating bushing i5. Item I6 is alsoan insulating bushing. The emitting electrode 5 is connected to ground,as shown. Intermediate electrode I2 is maintained at a unidirectionalpotential of around 800 volts relative to ground by means of potentialsource ll. Collecting electrode I3 is maintained at .a unidirectionalpotential of about 1500 volts relative tointermediate electrode I2 bymeans of potential source 18. The electrical condenser iii of 0.10microfarad capacity acts as an accumulator and facilitates the flow ofelectrical charges between emitting electrode 5 and collecting electrodel3. Resistor 36 of 2000 ohms is for current limiting purposes in case oftemporary fluid bridges grounding electrode l2. A source 20 of highfrequency current at about 50,000 cycles per second is connected toprimary coupling coil 2|. A secondary winding 22 coupled with coil 2!introduces a high frequency potential in series between collectingelectrode 13 and direct current potential source l8.

The dimensions of the apparatus shown in Fig. l for the most part arenot critical. Vessel I may be 6 inches in diameter measured horizontallyand electrode 5 may be l inches in diameter. For the interelectrodepotential differences specified, I prefer a minimum spacing betweenemitting electrode 5 at its nearest flexed position and intermediateelectrode I2 of inch, and between intermediate electrode l2 andcollecting electrode l3 of 1 /2 inch.

Operation of the device shown in Fig. 1 is as follows: A gas to bereacted such as propane, for example enters through gas inlet 2 at lbs.13. s. i. g. pressure and about 85 6. temperature. The propane gaspasses downward through collecting screen electrode 13 and leavesthrough outlet 3'. The emitting electrode 5 projects a cloud of liquidbutane spray particles at the reaction zone pressure of 165 lbs. p. s.i. g. The li uid butane would be at about 65 C. temperature and would beprojected as spray from electrode 5 during periods of verticalvibration. The liquid butane particles projected downward carry anelectric charge due to the electrostatic inducti h efiect of andelectrode 2 nd collecting trode l3. "After passing downward through theintermediate grid electrode l2 the charged butane particles mix with thepropane gas entering through connection 2. At the same time the electriccharges carried on the particles are subjected to the high frequencyelectrostatic field set up between grid electrode 12 and collectingelectrode l3. Gasification of the butane spray particles occurs at areaction zone temperature of about 95 C. due partly to heat transferfrom the propane gas, partly to heat generated by high frequencycirculating currents and partly to reaction heat evolved in surroundinggas. Ionization and local electrolytic action also take place in the gasmixture which is in the reaction zone. Polymerization products resultingfrom this action may be collected as condensate'in the bottom of vessel1 or they may be separated from the gas leaving the apparatus by meansthat do not form a part of this invention. Between periods of vibrationof the emitting electrode 5, the lower surface of electrode 5 is rewetwith fluid entering through the tube 8. Residual electric charges arecollected largely by electrode I3 and returning through the externalcircuit to emitting electrode 5. Flow rates may be 8 lbs. per hour ofliquid butane to 600 std. cu. ft. per hour of propane gas.

In Fig. 2 the vessel I also is of electrically nonconducting material asin Fig. 1. Likewise, a gas inlet 2 and gas outlet 3 and drain connection4 are provided. An emitting electrode 5 is vibrated in a horizontaldirection by shaft 5 which passes through the gas-tight sleeve II and isconnected to the source I of intermittent vibratory motion. The emittingelectrode 5 is a 4 inch diameter flexible plate of metal provided withinch perforations to the extent of 40% of the plate area. Electrode 5 issupported at the edges by the insulating collar 23. Emitting electrode5' is supplied with fluid used to form charged particles through thetube 8 which makes a right angle bend and extends horizontally acrossthe top of emitting electrode 5. A slot 9 is provided in the horizontalportion of tube 8 close to the surface of emitting electrode 5. Inbetween periods of vibration of electrode 5 the fluid supplied throughtube 8 and slot 9 runs down over the front surface of emitting electrode5. The intermediate grid electrode 12 and collecting screen electrode [3are similar to those in Fig. l and function in the same manner exceptthat they do not set up any high frequency electrostatic field. Vessel Imay be 6 inches in diameter measured vertically. The spacings betweenelectrodes 5, I 2 and 13 may be the same as in Fig. l. The parallelplate electrodes 24 and 25 which are spaced approximately 5 inches apartare connected through insulating bushings 26 and 21 to the highfrequency secondary winding 22. The source 20 of high fre quency currentand primary winding 2| are the same as in Fig. 1. The emitting electrode5 is connected to ground. Direct current potentials l1 and I8 andelectrical condenser l9 and resistor 36 are the same as in Fig. l. Thehigh frequency electrodes 24 and 25 are maintained at a negative directcurrent potential of about I 50 volts relative to ground by potentialsource 39.

' Operation of the device shown in Fig. 2 is very similar to that ofFig. 1. The gas or suspension .of material in a gas to be reacted entersthrough inlet 2, passes through the perforations in emitting electrode 5toward the grid electrode l2 and collecting screen electrode 13 and outthrough the connection 3. At the same time, charged particles of. thefluid supplied through the tube Bare projectedfrom emitting electrode 5through the intermediate grid electrode l2 and toward the collecting's'creen electrode I3. Circulating currents and electrolytic action inthe mixture of charged particles and gas or suspension is promoted bythe high frequency electrostatic field set up between electrodes 24 and25. If, as in Fig. 1, propane gas were introduced through inlet 2 andliquid butane through tube 8, the same pressures and temperatures wouldbe used as in Fig. 1, also the same flow rates and vibration cycle.

' It may be desirable to make use of a perforated emitting electrodesuch as has'been described in connection-with Fig. 2 and to circulatethe gaseous substances to be reacted counter-current to the projectionof electrically charged spray particles, at the sametime connecting thehigh frequency potential between the intermediate grid electrode andcollecting electrode as in Fig. 1. In this case, referring to Fig. 2,the gaseous substances to be reacted would enter the apparatus throughconnection 3' and exit gas including some reaction products would leavethe apparatus through connection 2. The high frequency potential winding22 would be connected into the lead to electrode l3, as it is shown inFig. 1. Potential 39 and its ground connection would be omitted. Liquidreactant would enter at 8 and would be projected as spray particles fromthe surface of emitting electrode 5 toward electrodes l2 and is aspreviously described. Such an arrangement appears to be advantageoussince the gaseous reactant substances would be intimately mixed with theprojected electrically charged spray particles of liquid reactantimmediately upon these spray particles leaving the surface of theemitting electrode, minimizing the distance that these charged sprayparticles must be projected. This eifect could be carried even furtherby connecting the high frequency potential between the emittingelectrode 5 and the intermediate grid electrode 12. With counter-currentflow of the gaseous reactant and electrically charged spray particles,gas ions and electrically charged products may not travel all the way tothe collecting electrode. A reversal of the direction of travel may takeplace with the electric charges ultimately reaching the intermediategrid electrode and the discharged products passing out of the reactionzone through the perforations in the emitting electrode. Variation ofthe potential of the collecting electrode [3 enables this to becontrolled together with the velocity of the gaseous reactant throughthe apparatus to ob- ,tain the best operating conditions.

With such an arrangement for applying the high frequency electrostaticfield between electrodes i2 and i 3 in Fig. 2 which has just beendescribed for countercurrent flow, if liquid butane and propane gas werereacted the temperatures and pressures and reactant flow rates may bethe same as in Fig. 1.

In Fig. 3 the vessel I is constructed of electrically non-conductingmaterial as in Figures 1 and 2. Likewise, a gas inlet 2, processed gasoutlet 3 and drain outlet 4 are provided. The arrangement of theemitting electrode 5, its dimensions and the method of supplyin fluid toelectrode 5 from which charged particles are formed and means forvibrating the electrode are identical with those used in Fig. 1. Thefirst intermediate grid electrode I2 is identical with that of Fig. 1and serves the same purpose. Capacitance l9 andresistor 36 are the sameas in Fig." 1. In order to have the high frequency accuses winding 28 ata proper-distance from the emittin electrode and to avoid excessivecirculating currents in the emitting electrode, it is necessary to makeuse of several intermediate grid electrodes 29 and 30. These second andthird intermediate grid electrodes '29 and '30 as well as the collectingscreen electrode 13 arefshaped as shown in Fig. 4 so as to discouragecirculating currents. If desired, electrode l2 can also be shaped asshown in Fig. 4. The unidirectional potentials 3|, 32 and 33 are each1500 volts. Unidirectional potential I! is 800 volts. The high frequencywinding 28, consisting-of 40 turns approximately 4. /2 inches indiameter, passes completely around the vessel I as shown and is suppliedwith high frequency current from the source .20 at a fre quency of about50,000 cycles per second. Items 15, I6, 3'! and 38 are insulatingbushings. Vessel i may be 4 inches in diameter where the winding 23passes around it. Electrode 12 may be inch from emitting electrode 5 inits nearest flexed position. The spacings between electrodes I2, 29, ccand it are each 1% inches.

Operation of the device shown in Fig. 3 is as follows: The gas to bereacted, such as propane for example, enters through the .gas inlet 2and mixes with the electrically charged particles of liquid butane, forexample, which are projected downward from the lower surface ofelectrode 5. as in Fig. l. Pressures and temperatures of the tworeactants may be the same as in Fig. 1. The mixture of charged butaneparticles and propane gas travels downward through the intermediate gridelectrodes 29 and 30. As this mixture passes through the high frequencyelectromagnetic field set up by the winding 28, circulating currents areproduced throughout the mixture, resulting in increased ionization ofthe gas or suspension and local electrolytic action. Residual electriccharges equal to those leaving, the emitting electrode 5 are collectedprincipally on the screen electrode I3 and partially on the intermediate electrode [2 and are returned through the external circuitshown and various leakage paths to the emitting electrode 5.Polymerization products resulting may be'collected in the bottom ofvessel I or may be separated from the processed gas leaving throughoutlet 3 by separate condensing means not shown. Flow rates are the sameas in Fig. 1.

In Fig. 5 the alternative arrangemnet of the high frequency winding suchas is used in Fig. 3 consists merely of directing the electromagneticfield across the path of the charged particles and gas by splitting thewinding into two halves 34 and 35. Other parts of the construction wouldremain the same as in Fig. 3.

In Figures 1 and 3 there are shown electrical connections forcreatingspace charges of nega tive polarity. Opposite polarities of thepotential sources used .will create positive space charges as readily asnegative ones. The size of the po'- tentials applied between the variouselectrodes and the rate of vibration or rotation of certain emittingelectrodes are not critical but can be varied as desired.

In Fig. 6 is shown an alternative arrangement with a rotating emittingelectrode which can be used in place of the vibratory emittingelectrodes shown in Figures 1 and 3. A partial sectional view only isshown in which item I is the wall of the Vessel, H is a gas-tightinsulating bushing which allows rotation of the shaft 8 and a discemitting electrode 5 attached thereto. Item in is a'motor which. turns.hart. 6 at approxt mately .200 R. P. M. Tube 8 feeds fluid material tothe top surface of disc 5 and the material then projected in the form offine particles from the edge'of the disc 5 and falls through the-openings in the intermediate grid electrode 12-. Item i5 is an insulatingbushing.

With regard to the electrical processing of sus pensions in gases, it iscontemplated thatcertain' materials in a finely divided state may besuspended in a gas in order to be able to process them in electric spacecharge apparatus. The gas present may or may not enter into the reactionor change of state which it is desired to accomplish.

As mentioned in my copending applications, it

may be desirable to use insulating bushings and electrode supports whichare provided with in" ternal heating coils so as to prevent wetting ofthe insulating surfaces exposed inside the processing chamber. I

In my copending application No. 34,300 there is disclosed an emittingelectrode arrangement for electric space charge devices which isparticularly adapted to electrically charging and spraying highdielectric strength liquids. This arrangement is described as a liquidfilm charging arrangment, and consists of a close clearance passage withopposite electrode walls which produce a displacement type chargingcurrent in a liquid film which is passed through the close clearancepassage and issues from it as a spray directed toward intermediateelectrodes and a collecting electrode similar in principle to those usedin this application. The use of emitting electrode arrangements of thetype disclosed in my copending application No. 34,300 in combinationwith high frequency electric fields, as-herein disclosed, iscontemplated.

In the claims the expression emitting elec trode" is intended to coverbroadly any type of electrode for projecting mechanically orhydraulically material particles which are electrically charged due tothe functioning of the emitting electrode in combination with otherseparated electrodes in the apparatus.

Obviously, the electro-chemical reaction method which has beenillustrated is applicable to many vapor phase reaction processesnormally requiring material catalytic agents.- Eithe-r l.-1I-i-'saturated or saturated hydrocarbons can be polymerized and many othertypes of reactions accomplished between gasifiable' liquids or sol-idsand gases.

This invention has been illustrated only in a general preferred formthroughout and it should be understood that it is capable of many andvaried modifications without departing from its purpose and scope, and Itherefore believe my-; self to be entitled to make and use any and allof these modifications such as suggest themselves to those skilled inthe art to whichthe invention;

1 is directed, provided that such modifications fall fairly within thepurpose and scopeof the hereinafter appended claims.

Whatis claimed is: v y

1. A method of reacting a liquid and gaseous substances comprisingproviding a reactionzone with an emitting electrode, an intermediateelectrode and a collecting electrode; passing said gaseous substances tobe reacted through said zone while projecting electrically charged sprayparticles of said liquid substance from said emitting electrode towardsaid intermediate electrode and said'collecting electrode respectively;main-=- W n n a t r-med ee c r e an co l t;

ing electrode at unidirectional electric potential .cliiferencesrelative to emitting electrode pten tial which potential differencesprogressively increase along the path of said electrically charged sprayparticles, said unidirectional potential differences between saidelectrodes being limited to values such that direct interelectrodeunidirectional current discharging does not take place; subjecting saidgaseous substances and electrically charged spray particles of saidliquid substance to a high frequency electric field having a frequencyabove about 50,000 cycles per second; gasifying said electricallycharged spray particles of said liquid substance to produce ionized gasand concurrently causing a drift through said reaction zone of saidelectrically charged liquid spray particles, gas ions and electricallycharged reaction products towards said c01lecting electrode andwithdrawing the reaction products from said zone.

2. A method of reacting a liquid and gaseous substances comprisingproviding a reaction zone with an emitting electrode, an intermediateelectrode and a collecting electrode; passing said gaseous substances tobe reacted through said zone while projecting electrically charged sprayparticles of said liquid substance from said emitting electrode towardsaid intermediate electrode and said collecting electrode respectively;maintaining said intermediate electrode and collecting electrode atunidirectional electric potential differences relative to emittingelectrode potential which potential differences promote elec- 'emitting,intermediate and collecting electrodes being so spaced that the reactionis initiated principally in the region between sad intermediateelectrode and said collecting electrode; concurrently causing a driftthrough said reaction zone of said electrically charged liquid sprayparticles, gas ions and electrically charged reaction products towardsaid collecting electrode and withdrawing the reaction products fromsaid zone.

3. A method of reacting a liquid and gaseous substances comprisingproviding a reaction zone with an emitting electrode, an intermediateelectrode and a collecting electrode; passing said.

gaseous substances to be reacted through said zone while projectingelectrically charged spray particles of said liquid substance from saidemitting electrode toward said intermediate electrode and saidcollecting electrode respectively; maintaining. said intermediateelectrode and collecting electrode at unidirectional electric potentialdifferences relative to emitting electrode potential which potentialdifferences progressively increase along the path of said electricallycharged .spray particles, said unidirectional potential differencesbetween said electrodesbeing limited to values such that directinterelectrode unidirectional current discharging does not take place;subjecting said gaseous substances and electrically charged sprayparticles of said liquid substance to a high frequency electrostaticfield having a frequency above about 50,000 cycles per second; gasifyingsaid electrically charged spray particles of said liquid substance toproduce ionized gas and concurrently causing a drift through saidreaction zone of said electrically charged liquid spray particles gasions and electrically charged reaction products towards said collectingelectrode and withdrawing the reaction products from said zone.

4. A method of reacting a liquid and gaseous substances comprisingproviding a reaction zone with an emitting electrode, an intermediateelectrode and a collecting electrode; passing said gaseous substances tobe reacted through said zone while projecting electrically charged sprayparticles of said liquid substance from said emitting electrode towardsaid intermediate electrode and said collecting electrode respectively;maintaining said intermediate electrode and collecting electrode atunidirectional electric potential diiferences relative to emittingelectrode potential which potential differences progressively increasealong the path of said electrically charged spray particles, saidunidirectional potential differences between said electrodes beinglimited to values such that direct interelectrode unidirectional currentdischarging does not take place; subjecting said gaseous substances andelectrically charged spray particles of said liquid substance to ahigh'frequency electromagnetic field i having a frequency above about50,000 cycles per second; gasifying said electrically charged sprayparticles of said liquid substance to produce ionized gas andconcurrently causing a drift through said reaction zone of saidelectrically charged liquid spray particles, gas ions and electricallycharged reaction products towards said collecting electrode andwithdrawing the reaction products fromlsaid zone.

5. A method of reacting a liquid and gaseous substances comprisingproviding a reaction zone with an emitting electrode, an intermediateelectrode and a collecting electrode; passing said gaseous substances tobe reacted through said zone while projecting electrically charged sprayparticles of said liquid substance from said emitting electrode towardsaid intermediate electrode and said collecting electrode respectively;maintaining said intermediate electrode and collecting electrode atunidirectional electric potential differences relative to emittingelectrode potential which potential differences progressively increasealong the path of said electrically charged spray particles, saidunidirectional potential differences between said electrodes beinglimited to values such that direct'interelectrode unidirec- -tionalcurrent discharging does not take place; subjecting said gaseoussubstances and electrically charged spray particles of said liquidsubstance to a high frequency electric field having a frequency aboveabout 50,000 cycles per second'; gasifying said electrically chargedspray particles of said liquid substance thereby dispersing intosurrounding gas the electric charges carried on said spray particles andconcurrently causing a drift through said reaction zone of saidelectrically charged liquid spray particles, gas ions and electricallycharged reaction products towards said collecting electrode andwithdrawing the reaction products from said zone. v 6. A method ofreacting a liquid and'gaseous substances comprising providing a reactionzone with an emitting electrode, an intermediate eleo-' l1 trode and acollecting electrode; passing said gaseous substances to be reactedthrough said zone While projecting electrically charged spray particlesof said liquid substance from said emitting electrode toward saidintermediate electrode and said collecting electrode respectively;maintaining said intermediate electrode and collecting' electrode atunidirectional electric potential differences relative to emittingelectrode potential which potential differences progressively increasealong the path of said electrically charged spray particles, saidunidirectional potential differences between said electrodes beinglimited to values such that direct interelectrode unidirectional currentdischarging does not take place; subjecting said gaseous substances andelectrically charged spray particles of said liquid substance to a highfrequency electric field having a frequency above about 50,000 cyclespersecond for the purpose of gasifying and ionizing said liquidsubstance and producing circulating currents in the gas mixture, saidemitting, intermediate and collecting electrodes being so'spaced thatthe reaction is initiated principally in the region between saidintermediate electrode and said collecting electrode; andconcurrently'causing a drift through said reaction zone of saidelectrically charged liquid spray particles, gas ions and electricallycharged reaction products towards said collecting electrode andwithdrawing the reaction products from said zone.

7. A method of reacting a liquid hydrocarbon and a gaseous hydrocarboncomprising providing a reaction zone with an emitting electrode,anintermediate electrode and a col ectin el ctrode; passing said gaseoushydrocarbon through said zone while projecting electrically chargedspray particles of said liquid hydrocarbon from said emitting electrodetoward said intermediate electrode and said collecting electroderespectively; maintaining said intermediate electrode and collectingelectrode at unidirectional electric potential differences relative toemitting electrode potential which potential difierences progressivelyincreaseal'ong the path of said electrically charged spray particles,said unidirectional potential' differences between said electrodes beinglimited to values such that direct interelectrode unidirectional currentdischarging does not take place; subjecting said gaseous hydrocarbon andelectrically charged spray particles of said liquid hydrocarbon to ahigh frequency electric field having a frequency above about 50,000cycles per second for the purpose of gasifying and ionizing saidliquidhydrocarbon and producing circulating currents in the gas mixture, saidemitting, intermediate and collecting electrodes being sospaced that thereaction is initiated principally in the region between saidintermediate electrode and said collecting electrode; and concurrentlycausing a drift through said reaction zone of said electrically chargedliquid hydrocarbon spray particies, gas ions and electrically chargedreaction products towards said collecting electrode and withdrawing thereaction products from saidzone.

8. A method of reacting liquid butane and propane gas comprisingproviding a reaction zone with. an emitting electrode, an intermediate618C,- trode and a collecting electrode; passing said propane gasthrough said zone while projecting electrically charged spray particlesof said. liquid butane from said emitting electrode toward saidintermediate electrode and said collecting electrode respectively;maintaining said intermediate electrode and collecting electrode atunidirem,

ti'onal electric potential differences relative to emitting electrodepotential which potential differences progressively increase along thepath of said electrically charged spray particles, said unidirectional.potential differences between said eliectrodesbeing limited to. valuessuch that direct interelectrode unidirectional current discharging doesnot take place; subjecting said propane gas and electrically chargedspray particles of said liquid; butane to a high frequency electricfield having; a frequency above about 50,000 cycles per second for thepurpose of gasifying and ionizing said liquid butane and producingcirculating currents: in the gas mixture, said emitting, intermediateand collecting electrodes being so spaced that the reaction is initiatedprincipally in the region between'said intermediate electrode and saidcollecting electrode; and concurrently causing a drift through saidreaction zone of said electrically charged liquid butane sprayparticles, gas ions and electrically charged reaction products towardssaid collecting electrode and withdrawing the reaction products fromsaid zone.

9. A method of reacting a liquid and gaseous r substances comprisingproviding a reaction zone with a perforated emitting electrode, anintermediate electrode and a collecting electrode; projectingelectrically charged spray particles of said liquid substance from saidemitting electrode toward said intermediate electrode and said collecting, electrode respectively; maintaining said intermediate electrodeand collecting electrode at unidirectional electric potentialdifferences relative to emitting electrode potential which potential,differences progressively increase along the path of said electricallycharged spray particles,v said unidirectional potential differencesbetween said electrodes being limited to values such that directinterelectrode unidirectional current discharging, does not take place;passing said gaseous substances to be reacted through said zone andvthrough the perforations in said emitting electrode countercurrent tothe projection of said electrically charged spray particles from saidemitting electrode; subjecting said gaseous substances and. electricallycharged spray particles of said liquid substance to a high frequencyelectric field having a frequency above about 50,000 cycles per second;gasifying said electrically charged spray particles of said liquidsubstance to produce ionized gas and concurrently causing an initialdrift of said electrically charged liquid spray particles, gas ions andelectrically charged reaction products towards said collecting electrodedue to said interelectrode unidirectional potential differences andwithdrawing the reaction, products from said zone.

LESTER H. SMITH.

REFERENCES CITED The following references are of record in the file ofthis patent:

UNITED STATES PATENTS Number Name Date 1,930,964: Bethenod Oct. 17, 19332,301,315 Opp Nov. 10, 1942 2,334,377 Bennett Nov. 16, 1943 FOREIGNPATENTS Number Country Date 2941,099 Great Brtiain June 20, 1929 421,811Great Britain Dec. 20, 1934 {302,063 Great Britain Mar. 10, 1939

1. A METHOD OF REACTING A LIQUID AND GASEOUS SUBSTANCES COMPRISINGPROVIDING A REACTION ZONE WITH AN EMITTING ELECTRODE, AN INTERMEDIATEELECTRODE AND A COLLECTING ELECTRODE; PASSING SAID GASEOUS SUBSTANCES TOBE REACTRED THROUGH SAID ZONE WHILE PROJECTING ELECTRICALLY CHARGEDSPRAY PARTICLE OF SAID LIQUID SUBSTANCE FROM SIAD EMITTING ELECTRODETOWARD SAID INTERMEDIATE ELECTRODE AND SAID COLLECTING ELECTRODERESPECTIVELY; MAINTAINING SAID INTERMEDATE ELECTRODE AND COLLECINGELECTRODE AT UNIDIRECTIONAL ELECTRIC POTENTIAL DIFFERENCES RELATIVE TOEMITTING ELECTRODE POTENTIAL WHICH POTENTIAL DIFFERENCES PROGRESSIVELYINCREASE ALONG THE PATH OF SAID ELECTRICALLY CHARGED SPRAY PARTICLES,SAID UNIDIRECTIONAL POTENTIAL DIFFERENCES BETWEEN SAID ELECTRODES BEINGLIMITED TO VALUES SUCH THAT DIRECT INTERELECTRODE UNIDIRECTIONAL CURRENTDISCHARGING DOES NOT TAKE PLACE; SUBJECTING SAID GASEOUS SUBSTANCES ANDELECTRICALLY CHARGED SPRAY PARTICLES OF SAID LIQUID SUBSTANCE TO A HIGHFREQUENCY ELECTRIC FIELD HAVING A FREQUENCY ABOVE ABOUT 50,000 CYCLESPER SECOND; GASIFYING SAID ELECTRICALLY CHARGED SPRAY PARTICLES OF SAIDLIQUID SUBSTANCES TO PRODUCE IONIZED GAS AND CONCURRENTLY CAUSING ADRIFT THROUGH SAID REACTION ZONE OF SAID ELECTRICALLY CHARGED LIQUIDSPRAY PARTICLES, GAS IONS AND ELECTRICALLY CHARGED REACTION PRODUCTSTOWARDS SAID COLLECTING ELECTRODE AND WITHDRAWING THE REACTION PRODUCTSFROM SAID ZONE.